Crosslinking agents, notably sulfur, are used in asphalt binder modification to facilitate chemical bonding between polymer chains and the asphalt binder. Despite some prior research indicating the benefits of sulfur crosslinking in enhancing polymer-modified asphalt’s (PMA) stability, there is a lack of comprehensive understanding regarding its impact on rheological properties and its anti-aging potential. This study addresses these gaps by thoroughly investigating the effects of varying the sulfur content (ranging from 0.03% to 0.5% by total weight of binder) on PMA’s rheological properties. The research assesses the effectiveness of sulfur in enhancing PMA’s resistance to aging using various methods, including the Glover-Rowe parameter, FTIR analysis, and the examination of the dynamic modulus and phase angle master curves. The results indicated that the addition of sulfur, particularly up to 0.3%, bumps the high-temperature performance grade by one level, and significantly improves elasticity, allowing the PMA to support heavier traffic without experiencing rutting, all while maintaining resistance to low-temperature cracking. Furthermore, PMA with sulfur demonstrated an increase in resistance to aging, reducing the aging potential by approximately 15% with the best sulfur formulation. This enhanced durability can reduce the frequency of maintenance activities, leading to cost savings, reduced roadwork emissions, and prolonged pavement life.